Unifying Theoretical Framework for Deciphering the Oxygen Reduction Reaction on Platinum

Resource type
Date created
2018-04-05
Authors/Contributors
Abstract
Rapid conversion of oxygen into water is crucial to the operation of polymer electrolyte fuel cells and other emerging electrochemical energy technologies. Chemisorbed oxygen species play double-edged roles in this reaction, acting as vital intermediates on one hand and site-blockers on the other. Any attempt to decipher the oxygen reduction reaction (ORR) must first relate the formation of oxygen intermediates to basic electronic and electrostatic properties of the catalytic surface, and then link it to parameters of catalyst activity. An approach that accomplishes this feat will be of great utility for catalyst materials development and predictive model formulation of electrode operation. Here, we present a theoretical framework for the multiple interrelated surface phenomena and processes involved, particularly, by incorporating the double-layer effects. It sheds light on the roles of oxygen intermediates and gives out the Tafel slope and exchange current density as continuous functions of electrode potential. Moreover, it develops the concept of a rate determining term which should replace the concept of a rate determining step for multi-electron reactions, and offers a new perspective on the volcano relation of the ORR.
Document
Description
Supplementary data is also included in a separate file.
Identifier
DOI: 10.1039/C8CP01315B
Published as
J. Huang, J.Zhang and M. Eikerling. Unifying theoretical framework for deciphering the oxygen reduction reaction on platinum. Physical Chemistry Chemical Physics, 2018, DOI: 10.1039/C8CP01315B
Publication title
Physical Chemistry Chemical Physics
Document title
Unifying Theoretical Framework for Deciphering the Oxygen Reduction Reaction on Platinum
Date
2018
Publisher DOI
10.1039/C8CP01315B
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Copyright is held by the author(s).
Scholarly level
Peer reviewed?
Yes
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orr_theory_v14_me.pdf 1018.82 KB